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The classical light interactions of nanosilicon, which is a dielectric material, are exceedingly weak for radius r ≪ λ (wavelength), scaling as r6. It exhibits geometrical anisotropy-based depolarization, which is the basis for the very weak response in isotropic structures (nanosphere). Recently, surface enhanced Raman scattering (SERS) in DNA decorated with ultrasmall Si nanoparticles has been demonstrated, affording an effective alternative to plasmon–metal particles. In this paper, we execute fundamental quantum atomistic computation of 1 nm hydrogenated Si particles, with different surface reconstruction and termination, including Si–H, H–Si–Si–H (dimer molecules), or oxygenated dimer bridges (H–Si–O–Si–H). We obtain the mechanical vibrational modes of the particles. Our results show that by changing the surface configuration one can control the symmetry and normal vibration modes, and enhance the polarizability, polarity, and light interactions (scattering, absorption, and depolarization/memory). The low frequency polarizability (Raman scattering) shifts spatially from the interior to the surface, while the infrared polarity remains on the surface, but its bandwidth narrows spectrally. The results support previous infrared absorption and light scattering and depolarization measurements, as well recent SERS, which enable Si nanoparticles to be an effective alternative to plasmonic metal particles. Molecular surface reconstruction in terms of Si dimers and bridges were suggested as the source of the novel nonlinear and anisotropic luminescence and photonic properties of Si nanoparticles. Such control affords potential for optimizing the design and operation of a wide range of opto-electronic advanced scattering and luminescence devices. [ABSTRACT FROM AUTHOR]